Electrochemical conversion of nitrate(NO_(3)^(-))to ammonia(NH_(3))appears to be a carbon-neutral method to handle wastewater remediation,while providing an innovative pathway for high-value green ammonia synthesis.Ho...Electrochemical conversion of nitrate(NO_(3)^(-))to ammonia(NH_(3))appears to be a carbon-neutral method to handle wastewater remediation,while providing an innovative pathway for high-value green ammonia synthesis.However,designing highly efficient electrochemical catalysts remains one of the primary challenges in fulfilling this strategy.Herein,we constructed a series of Cu@NxC metal-carbon Mott-Schottky heterostructures composed of Cu nanoparticles uniformly dispersed on tailorable N-doped carbon substrates.The broad range of the content of the N dopant greatly enables adjusting the band gap of the carbon.The increased N content leads to a higher degree of interfacial charge separation.The optimal heterostructured Cu@N1.0C electrocatalyst presents a FENH_(3)of 96.2%at−0.9 V vs.RHE and a remarkable NH_(3)yield of 1353.1 mmol h^(-1)gcat^(-1)at^(-1).1 V vs.RHE,superior to those of the reference Cu@C and most of the reported NO_(3)RR catalysts.The mechanism investigation demonstrates that rectifying Schottky contacts in the Cu@NxC heterostructures reduces the electron density of the Cu sites and further improves the Cu^(+)concentration,thus promoting the adsorption and activation of NO_(3)^(-).This study offers a new possibility for improving the NO_(3)RR performance of electrocatalysts by the rectification strategy.展开更多
基金supported by the National Natural Science Foundation of China(No.22278108 and 22008048)Natural Science Foundation of Tianjin(22JCYBJC00250)+2 种基金Natural Science Foundation for Outstanding Youth Scholars of Hebei Province(No.B2021202061)Natural Science Foundation of Hebei Province(No.B2021202010)State Key Laboratory of Fine Chemicals,Dalian University of Technology(KF 2108).
文摘Electrochemical conversion of nitrate(NO_(3)^(-))to ammonia(NH_(3))appears to be a carbon-neutral method to handle wastewater remediation,while providing an innovative pathway for high-value green ammonia synthesis.However,designing highly efficient electrochemical catalysts remains one of the primary challenges in fulfilling this strategy.Herein,we constructed a series of Cu@NxC metal-carbon Mott-Schottky heterostructures composed of Cu nanoparticles uniformly dispersed on tailorable N-doped carbon substrates.The broad range of the content of the N dopant greatly enables adjusting the band gap of the carbon.The increased N content leads to a higher degree of interfacial charge separation.The optimal heterostructured Cu@N1.0C electrocatalyst presents a FENH_(3)of 96.2%at−0.9 V vs.RHE and a remarkable NH_(3)yield of 1353.1 mmol h^(-1)gcat^(-1)at^(-1).1 V vs.RHE,superior to those of the reference Cu@C and most of the reported NO_(3)RR catalysts.The mechanism investigation demonstrates that rectifying Schottky contacts in the Cu@NxC heterostructures reduces the electron density of the Cu sites and further improves the Cu^(+)concentration,thus promoting the adsorption and activation of NO_(3)^(-).This study offers a new possibility for improving the NO_(3)RR performance of electrocatalysts by the rectification strategy.
